Article

 

Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC(4)RS) and ground-based (SOAS) observations in the Southeast US Public Deposited

https://scholar.colorado.edu/concern/articles/wd375w99w
Abstract
  • Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with similar to aEuro-25aEuro- x aEuro-25aEuro-km(2) resolution over North America. We evaluate the model using aircraft (SEAC(4)RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25-50aEuro-% of observed RONO2 in surface air, and we find that another 10aEuro-% is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10aEuro-% of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60aEuro-% of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20aEuro-% by photolysis to recycle NOx and 15aEuro-% by dry deposition. RONO2 production accounts for 20aEuro-% of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.
Creator
Date Issued
  • 2016-05-17
Academic Affiliation
Journal Title
Journal Issue/Number
  • 9
Journal Volume
  • 16
Dernière modification
  • 2019-12-05
Resource Type
Déclaration de droits
DOI
ISSN
  • 1680-7324
Language

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